Search Results (86)

Traditional covalently cross-linked solid-state electrolytes exhibit desirable mechanical durability but suffer from limited processability and recyclability due to their permanent network structures. Incorporating dynamic covalent bonds offers a promising solution to these challenges. In this study, we report a reprocessable and recyclable polymer electrolyte based on a dynamic ester bond network, synthesized from commercially available materials. Polyethylene glycol diglycidyl ether (PEGDE) and glutaric anhydride (GA) were cross-linked and cured in the presence of benzyl dimethylamine (BDMA), forming an ester-rich polymer backbone. Subsequently, 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) was introduced as a transesterification catalyst to facilitate network rearrangement. Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) was incorporated to establish efficient ion transport pathways. By tuning the cross-linking density and catalyst ratio, the electrolyte achieved an ionic conductivity of 1.89 × 10⁻⁵ S/cm at room temperature along with excellent reprocessability. Full article

This work presents the development of two vanillin-based vitrimer epoxy flax fibre-reinforced composites, with both the VER1-1-FFRC (a vitrimer-to-epoxy ratio of 1:1) and VER1-2-FFRC (a vitrimer-to-epoxy ratio of 1:2), via a vacuum-assisted resin infusion. The thermal and mechanical properties of the resulting vitrimer epoxy flax composites were characterised using thermal gravimetric analysis (TGA), differential scanning calorimetry (DSC), dynamic mechanical analysis (DMA), and mechanical four-point bending tests, alongside studies of solvent resistance and chemical recyclability. Both the VER1-1-FFRC (degradation temperature T_deg of 377.0 °C) and VER1-2-FFRC (T_deg of 395.9 °C) exhibited relatively high thermal stability, which is comparable to the reference ER-FFRC (T_deg of 396.7 °C). The VER1-1-FFRC, VER1-2-FFRC, and ER-FFRC demonstrated glass transition temperatures T_g of 54.1 °C, 68.8 °C, and 83.4 °C, respectively. The low T_g of the vitrimer composite is due to the low crosslink density in the vitrimer epoxy resin. Particularly, the crosslinked density of the VER1-1-FFRC was measured to be 319.5 mol·m⁻³, which is lower than that obtained from the VER1-2-FFRC (434.7 mol·m⁻³) and ER-FFRC (442.9 mol·m⁻³). Furthermore, the mechanical properties of these composites are also affected by the low crosslink density. Indeed, the flexural strength of the VER1-1-FFRC was found to be 76.7 MPa, which was significantly lower than the VER1-2-FFRC (116.2 MPa) and the ER-FFRC (138.3 MPa). Despite their lower thermal and mechanical performance, these vitrimer composites offer promising recyclability and contribute to advancing sustainable composite materials. Full article

As the global push for renewable energy intensifies, the materials used in the generation, transmission, and storage of renewable energy systems have come under scrutiny due to their environmental impact. In particular, crosslinked polymers are extensively utilized in these systems because of their excellent thermal, mechanical, and electrical properties. However, their non-recyclable nature and significant waste generation at the end of their service life present severe sustainability challenges. This review employs a citation network-based methodology to analyze the role of crosslinked polymers in renewable energy systems, with a focus mainly on two critical applications: (1) production, specifically in the manufacturing of wind turbine blades; and (2) transmission, where they are integral to high-voltage cable insulation. Our complex network analysis reveals the major themes within the field of sustainability, providing a structured approach to understanding the lifecycle challenges of crosslinked polymers. The first part explores the primary polymers used, their typical lifespans, and the environmental burden of generated waste. We then describe both traditional recycling strategies and innovative approaches, such as supercritical water processing and thermoplasticizing technologies, which offer potential solutions to mitigate these impacts. Finally, we highlight emerging reprocessable materials, including vitrimers, ionomers, and specialty thermoplastic alternatives, which provide recyclability while maintaining performance. This comprehensive assessment emphasizes the urgent need for innovation in polymer science to achieve a circular economy for renewable energy systems. Full article

The production of fibre-reinforced composites for use in applications such as type-4 pressure vessels for hydrogen storage is achieved through the use of a thermoset matrix. However, the recycling of thermosets presents a significant challenge due to the lack of established recycling methods. Epoxy-based vitrimers show thermoset characteristics during the manufacturing and utilisation phases but exhibit thermoplastic behaviour at elevated temperatures of 190 °C. This study investigates the industrial-scale production of carbon fibre reinforced vitrimers via a wet filament winding, as exemplified by a type-4 pressure vessel demonstrator. Processing conditions of industrial processes have yet to be applied to vitrimers; therefore, two vitrimer formulations are compared to a conventional epoxy thermoset. The processability and resulting composite quality of wound composites using these materials as matrices are compared. The mechanical properties of the composites are compared using an interlaminar shear strength test, demonstrating that the vitrimeric matrices exhibit 19.8% (23 °C) and 49.2% (140 °C) improved interlaminar strength. Consequently, the epoxy-based vitrimers investigated in this study can be employed as a direct replacement for the thermoset matrix in industrial-scale applications, with the potential for recycling the composite. To increase composite qualities, the winding process must be adapted for vitrimers, since a pore free composite could not be achieved. Full article

The development of sustainable epoxy vitrimers with outstanding mechanical strength and facile self-healing capabilities are of great significance for prolonging the lifespan and enhancing the reliability of electronic devices. In this study, we present a castor oil-derived epoxy vitrimer (ASB–ECO) featuring dual dynamic networks enabled by rationally designed ester–imine bonds and an aromatic Schiff base-conjugated crosslinker architecture. This molecular design strategy effectively enhances the mechanical properties of vegetable oil-based vitrimers and endows them with controllable self-healing capabilities under photothermal conversion. The 1.0-ASB–ECO system demonstrates dynamic characteristics with an activation energy (Ea) of 37.25 kJ/mol and a topological freezing transition temperature (Tv) of 123.13 °C. The material exhibits a photothermal conversion efficiency (ηPT = 61.42%) and can achieve a self-healing rate of 100% under visible-light radiation. In addition, 1.0-ASB–ECO displays a dielectric constant (Dk) of 5.54 and a loss tangent (Df) of 0.025 at 106 Hz. This study on biomass-based epoxy vitrimers presents a novel approach to developing electronic materials, achieving a combination of high mechanical performance, sustainability, and photothermal self-healing properties. Full article

Conventional epoxy thermosets, with irreversible crosslinking networks, cannot be reprocessed and recycled. Furthermore, the utilization of petroleum-based materials accelerates the depletion of non-renewable resources. The introduction of dynamic covalent bonds and the use of bio-based materials for thermosets can effectively address the above issues. Herein, a series of bio-based epoxy vitrimers with dynamic covalent imine bonds were synthesized via a simple solvent-free, one-pot method using vanillin-derived aldehyde monomers, 4,4-diaminodiphenylsulfone (DDS) and bisphenol F diglycidyl ether (BFDGE) as raw materials. The effect of crosslinking density, crosslinking structure and imine bond content on the resulting bio-based vitrimers was studied, demonstrating their excellent thermal properties, UV shielding and solvent resistance, as well as outstanding mechanical properties compared to those of the previously reported vitrimers. In particular, the cured neat resin of vitrimer had a maximum tensile strength of 109 MPa and Young’s modulus of 6257 MPa, which are higher than those of previously reported imine-based vitrimers. The dynamic imine bonds endow these vitrimers with good reprocessability upon heating (over 70% recovery) and degradation under acidic conditions, enabling recycling by physical routes and gentle degradation by chemical routes. This study demonstrates a simple and effective process to prepare high-performance bio-based and recycled epoxy thermosets. Full article

Epoxy-based vitrimers represent a paradigm shift in material science, offering an unprecedented combination of mechanical robustness, environmental sustainability, and reconfigurability. These dynamic polymer systems utilize associative dynamic covalent bonds (DCBs) such as transesterification to blend the structural integrity of thermosets with the recyclability and self-healing properties of thermoplastics. This unique combination makes vitrimers ideal candidates for high-performance applications in industries such as civil engineering, where material durability, repairability, and environmental compatibility are critical. Epoxy-based vitrimers, in particular, exhibit exceptional self-healing capabilities, allowing them to autonomously repair microcracks and damage, restoring mechanical properties under appropriate stimuli such as heat or light. Their recyclability further aligns with global sustainability goals by reducing material waste and lifecycle costs. Recent advancements have also integrated bio-based feedstocks and scalable manufacturing methods, enhancing the feasibility of these materials for industrial applications. This review explores the underlying self-healing mechanisms, dynamic recycling processes, and the emerging role of epoxy-based vitrimers in civil engineering. Challenges related to scalability, mechanical optimization, and regulatory acceptance are also discussed, with a focus on their potential to drive sustainable innovation in infrastructure materials. Full article

To fulfill the current circular economy concept, the academic and industrial communities are devoting significant efforts to plastic materials’ end-of-life. Unlike thermoplastics, which are easy to recover and re-valorize, recycling thermosets is still difficult and challenging. Conversely, because of their network structure, thermosetting polymer systems exhibit peculiar features that make these materials preferable for several applications where high mechanical properties, chemical inertness, and thermal stability, among others, are demanded. In this view, vitrimers have quite recently attracted the attention of the scientific community, as they can form dynamic covalent adaptive networks that provide the properties typical of thermosets while keeping the possibility of being processed (and, therefore, mechanically recycled) beyond a certain temperature. This review aims to provide an overview of vitrimers, elucidating their most recent advances and applications and posing some perspectives for the forthcoming years. Full article

Carbon-fiber-reinforced polymers (CFRPs) with epoxy matrices are widely applied in high-performance structural applications and represent one of the biggest classes of materials with urgent need for end-of-life management. Available waste management methodologies for conventional thermoset composites with a focus on CFRPs are briefly reviewed and their limitations are highlighted. In the quest to obtain materials with mechanical performance, thermal stability, and sustainability, the research community has turned its interest to develop polymer composites with adaptable and dynamic networks in their matrix, and lately also at an interface/interphase level. The current review focuses on the life extension/waste management options that are opened through the introduction of covalent adaptable networks in the epoxy matrix of CFRPs. The processing conditions that are applied for the healing/repairing, welding/reshaping, and/or recycling of CFRPs are presented in detail, and compared based on the most common dynamic exchange reactions. Full article

The welding behavior of prototype vitrimer composites with respect to adjustable parameters and protocols is investigated, and a method for resistance welding of vitrimer composites directly adapted from the welding of thermoplastic composites is described. Adherend laminates are positioned on either side of a matrix-saturated carbon fiber heating element, through which current is driven, and resistance heating welds the adherends and heating element together, forming a single lap joint. Weld strengths matched or exceeded the strength of composite parts produced using the manufacturer-recommended consolidation method (12.0 ± 2.6 MPa vs. 8.4 ± 0.6 MPa). Furthermore, repeating the welding process yielded greater shear strength, withstanding up to five weld–break–reweld cycles with an average increase of 4.6 ± 1.5 MPa or 65% compared to the first weld. The findings from resistance weld experiments highlight the suitability of vitrimer matrix composites for repair. Finally, a process for reversing a welded joint was shown, demonstrating the potential for vitrimers for temporary joining and rejoining. Full article

Introducing dynamic ester bonds into epoxy–anhydride resins enhances the reprocessability of the crosslinked network, facilitated by various types of transesterification catalysts. However, existing catalysts, such as metal salts and organic molecules, often struggle with dispersion, volatility, or structural instability issues. Here, we propose to solve such problems by incorporating a liquid-state, thermally stable transesterification catalyst into epoxy resins. This catalyst, an imidazole derivative, can be uniformly dispersed in the epoxy resin at room temperature. In addition, it shows high-temperature structural stability above at least 200 °C as the synergistic effects of the electron-withdrawing group and steric bulk can be leveraged. It can also effectively promote transesterification at elevated temperatures, allowing for the effective release of shear stress. This property enables the thermal recycling and reshaping of the fully crosslinked epoxy–anhydride resin. This strategy not only enhances the functionality of epoxy resins but also broadens their applicability across various thermal and mechanical environments. Full article

Nowadays, self-healing materials have been studied actively in electronics, soft robotics, aerospace, and automobiles because they can prolong the life span of the materials. However, overcoming the trade-off relationship between mechanical properties and self-healing performance is challenging. Herein, graphene oxide-polyaniline (GO-PANI) filler was introduced to overcome this challenge because GO has a highly excellent modulus, and nitrogen atoms in PANI can endow a self-healing ability through hydrogen bonds. Aside from the hydrogen bond in PANI, the hydrogen bond in the carbonyl group and the disulfide exchange bond in the epoxy matrix also helped the materials heal efficiently. Therefore, the modulus of SV-GPN1 (Self-healing Vitrimer-GO-PANI1) reached 770 MPa, and a 65.0% healing efficiency was demonstrated. The modulus and self-healing efficiency were enhanced after adding GO-PANI filler. The self-healing ability, however, deteriorated when adding more GO-PANI filler because it hindered the collision between the molecules. Meanwhile, SV-GPN1 was excellent in reproducibility, which was proven by the experiment that 16.50 mm thick SV-GPN1 also displayed a self-healing ability. Thus, SV-GPN1 can be applied to structural materials in industries like aerospace because of its self-healing ability, excellent modulus, and reproducibility. Full article

As one of the most widely used thermosets due to its excellent performances, epoxy resin (EP) is widely used in various fields and often employed as a component of composite actuator devices, strengthening their mechanical properties. However, the expanding production of EP inevitably leads to the accumulation of waste end-of-life equipment and the corresponding increasingly serious environmental problems. This review summarizes the recycling strategies of EP, divided into two perspectives: recycling from wastes and sources. Chemical recycling is expected to be the future of waste EP treatment, and we discuss the chemical recycling methods of existing waste EP based on different mechanisms, including the selective cleavage of ester bonds, C–N bonds, and C–O bonds. On the other hand, epoxy vitrimer networks based on various dynamic covalent linkages are also outlined, which can respond to multiple external stimuli and provide materials with recyclability from the origin. Therefore, the use of epoxy vitrimer actuators can prevent waste generation throughout the whole lifecycle. We present some issues of concern in both waste-based and source-based recycling strategies and emphasize the significance of scaling-up. Finally, we summarized the current situation and present some future perspectives with the aim of making practical contributions to environmental issues. Full article

Recently, the growth of the recyclability of carbon fiber reinforced polymer (CFRP) composites has been driven by environmental and circular economic aspects. The main aim of this research work is to investigate the strength retention of a bio-based vitrimer composite reinforced with carbon fibers, which offers both recyclability and material reusability. The composite formulation consisted of an epoxy resin composed of diglycidyl ether of bioshpenol A (DGEBA) combined with tricarboxylic acid (citric acid, CA) and cardanol, which was then reinforced with carbon fibers to enhance its performance. Differential scanning calorimetry (DSC) and Fourier transform infrared (FTIR) spectroscopy were performed to analyze the chemical composition and curing behavior of the vitrimer. Mechanical testing under tensile loading at room temperature was carried out on epoxy, vitrimer, and associated carbon fiber reinforced composite materials. The results demonstrated that the DGEBA/CA/cardanol vitrimer exhibited thermomechanical properties comparable to those of an epoxy cured with petroleum-based curing agents. It was observed that the maximum tensile strength of vitrimer is about 50 MPa, which is very close to the range of epoxy resins cured with petroleum-based curing agents. Notably, the ability of the vitrimer composite to be effectively dissolved in a dimethylformamide (DMF) solvent is a significant advantage, as it enables the recovery of the fibers. The recovered carbon fiber retained comparable tensile strength to that of the fresh carbon composites. More than 95% strength was retained after the first recovery, which confirms the use of fibers for primary and secondary applications. These research results open up new avenues for efficient recycling and contribute to the overall sustainability of the composite material at an economic level. Full article

Classical viscoelastic models usually only consider the motion of chain segments and the motion of the entire molecular chain; therefore, they will cause inevitable errors when modeling self-healing vitrimer materials with many group movements. In this paper, a group-enriched viscoelastic model is proposed for self-healing vitrimers where the group effect cannot be neglected. We synthesize a specific damping vitrimer with many dangling chains, surpassing the limited loss modulus of conventional engineering materials. Due to the dangling chains, the damping capability can be improved and the group effect cannot be neglected in the synthesized damping vitrimer. The group-enriched viscoelastic model accurately captures the experimental damping behavior of the synthesized damping vitrimer. Our results indicate that the group-enriched viscoelastic model can improve the accuracy of classical viscoelastic models. It is shown that the group effect can be ignored at low frequencies since the chain segments have sufficient time for extensive realignment; however, the group effect can become significant in the case of high frequency or low temperature. Full article